Liu Xigui, Huang Danlian, Lai Cui, Qin Lei, Liu Shiyu, Zhang Mingming, Fu Yukui
Institute of Environmental Research at Greater Bay Area, Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Guangzhou University, Guangzhou 510006, Guangdong, PR China; College of Environmental Science and Engineering, Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha 410082, Hunan, PR China.
College of Environmental Science and Engineering, Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Changsha 410082, Hunan, PR China.
J Colloid Interface Sci. 2023 Jan;629(Pt B):417-427. doi: 10.1016/j.jcis.2022.08.108. Epub 2022 Aug 19.
As one of the tactics to produce reactive oxygen radicals, the Fenton-like process has been widely developed to solve the increasingly severe problem of environmental pollution. However, establishing advanced mediators with sufficient stability and activity for practical application is still a long-term objective. Herein, we proposed a facile strategy through polymeric carbon nitride (pCN) in-situ growth single cobalt atom for efficient degradation of antibiotics by peroxymonosulfate (PMS) activation. X-ray absorption spectroscopy and high-angle annular dark field-scanning transmission electron microscopy prove the single cobalt atoms are successfully anchored on pCN. Moreover, extended X-ray absorption fine structure analysis shows that the embedded cobalt atoms are constructed by covalently forming the Co-N bond and Co-O bond, which endow the single-atom cobalt catalyst with high stability. Experiment results indicate that the prepared single-atom cobalt catalyst can be used for efficient PMS activation catalytic degradation of tetracycline with a high degradation rate of 98.7 % in 60 min. And the CoN/O sites with single cobalt atoms serve as the active site for generating active radical species (singlet oxygen) from PMS activation. This work may expand the strategy for constructing single-atom catalysts and extend its application for the advanced oxidation process.
作为产生活性氧自由基的策略之一,类芬顿过程已得到广泛发展,以解决日益严重的环境污染问题。然而,开发具有足够稳定性和活性的先进催化剂用于实际应用仍然是一个长期目标。在此,我们提出了一种简便的策略,即通过聚合物氮化碳(pCN)原位生长单钴原子,以通过过一硫酸盐(PMS)活化高效降解抗生素。X射线吸收光谱和高角度环形暗场扫描透射电子显微镜证明单钴原子成功锚定在pCN上。此外,扩展X射线吸收精细结构分析表明,嵌入的钴原子通过共价形成Co-N键和Co-O键构建,这赋予了单原子钴催化剂高稳定性。实验结果表明,制备的单原子钴催化剂可用于高效PMS活化催化降解四环素,在60分钟内降解率高达98.7%。具有单钴原子的CoN/O位点作为从PMS活化产生活性自由基物种(单线态氧)的活性位点。这项工作可能会扩展构建单原子催化剂的策略,并将其应用扩展到高级氧化过程。